WO2020177760A1 - Électrode négative et batterie secondaire et dispositif les comprenant - Google Patents

Électrode négative et batterie secondaire et dispositif les comprenant Download PDF

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WO2020177760A1
WO2020177760A1 PCT/CN2020/078166 CN2020078166W WO2020177760A1 WO 2020177760 A1 WO2020177760 A1 WO 2020177760A1 CN 2020078166 W CN2020078166 W CN 2020078166W WO 2020177760 A1 WO2020177760 A1 WO 2020177760A1
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active material
negative electrode
material layer
secondary battery
battery
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PCT/CN2020/078166
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English (en)
Chinese (zh)
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郭明奎
王天生
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宁德时代新能源科技股份有限公司
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Priority to EP22168100.0A priority Critical patent/EP4047681B1/fr
Priority to EP20766175.2A priority patent/EP3800706B1/fr
Publication of WO2020177760A1 publication Critical patent/WO2020177760A1/fr
Priority to US17/150,096 priority patent/US11600816B2/en
Priority to US18/103,531 priority patent/US20230170474A1/en

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/134—Electrodes based on metals, Si or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/386—Silicon or alloys based on silicon
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • This application belongs to the technical field of energy storage devices, and specifically relates to a negative electrode, a secondary battery, and a device containing the secondary battery.
  • the secondary battery represented by the lithium ion secondary battery completes the charging and discharging process through the reciprocating insertion and extraction of active ions between the positive and negative active materials, and has become an important energy source.
  • the market demand for power-type secondary batteries will show explosive growth. While this brings opportunities for the development of the secondary battery industry, it also poses a severe challenge to the cycle life of the secondary battery. In order to enhance the market competitiveness of secondary batteries, it is indeed necessary to increase their cycle life.
  • the design of the negative electrode will directly affect the performance of the secondary battery.
  • the current negative electrode usually has a uniform negative electrode film on one or both sides of the current collector.
  • the inventor’s research has found that the negative electrode swells during the battery cycle, resulting in insufficient electrolyte infiltration, which causes the battery’s capacity to rapidly decay.
  • the inventors further found that by reducing the tightness of the active material particles in the negative electrode to improve the liquid absorption capacity of the negative electrode, the cycle life of the secondary battery can be improved. However, this will result in an increase in the thickness of the negative electrode, which will disadvantageously reduce the energy density of the secondary battery. In addition, there may also be a problem of poor contact between the active material particles, which affects the electron conduction of the negative electrode, thereby reducing the dynamic performance of the secondary battery.
  • the electrode can maintain a sufficient electrolyte content during the cycle, so that although the cycle life of the secondary battery can be improved to a certain extent, a higher content is added
  • the electrolyte will increase the internal pressure of the battery, which will cause the problem of battery cycle expansion and affect the safety performance of the battery.
  • using more electrolyte also increases battery cost.
  • the inventor has conducted a lot of research to improve the traditional negative electrode, so that the negative electrode can increase its own liquid absorption and storage capacity while having good accumulation performance of active material particles, so as to obtain a high A secondary battery with energy density and cycle life.
  • a negative electrode which includes:
  • the first active material and the second active material are each independently oval-like particles with through holes and/or blind holes, and the average pore diameter of the first active material is larger than the average of the second active material Aperture.
  • a second aspect of the present application provides a secondary battery including the negative electrode according to the first aspect of the present application.
  • a third aspect of the present application provides a device including the secondary battery according to the second aspect of the present application.
  • the negative electrode of the present application adopts a composite layer structure of the negative electrode film, wherein the first active material in the first active material layer and the second active material in the second active material layer have through holes and/or Oval-shaped particles with blind holes, and the average pore diameter of the first active material is larger than the average pore diameter of the second active material, which enables the negative electrode to have a good accumulation of active material particles while greatly increasing its own liquid absorption Liquid storage capacity. Therefore, the negative electrode of the present application enables the secondary battery using it to increase the cycle life on the premise of higher energy density.
  • the device of the present application includes the secondary battery provided by the present application, and therefore has at least the same advantages as the secondary battery.
  • FIG. 1 is a schematic diagram of a negative electrode structure provided by some embodiments of the application.
  • Fig. 2 is a schematic diagram of an embodiment of a secondary battery.
  • Fig. 3 is an exploded view of Fig. 2.
  • Fig. 4 is a schematic diagram of an embodiment of a battery module.
  • Fig. 5 is a schematic diagram of an embodiment of a battery pack.
  • Fig. 6 is an exploded view of Fig. 5.
  • Fig. 7 is a schematic diagram of an embodiment of a device in which a secondary battery is used as a power source.
  • any lower limit may be combined with any upper limit to form an unspecified range; and any lower limit may be combined with other lower limits to form an unspecified range, and any upper limit may be combined with any other upper limit to form an unspecified range.
  • every point or single value between the end points of the range is included in the range. Therefore, each point or single numerical value can be used as its own lower limit or upper limit in combination with any other point or single numerical value or in combination with other lower or upper limits to form an unspecified range.
  • the negative electrode includes: a negative electrode current collector; a first active material layer close to the negative electrode current collector, the first active material layer containing a first active material; and a first active material layer disposed on the first active material layer away from the negative electrode current collector
  • the second active material layer on the surface of the second active material layer contains a second active material; the first active material and the second active material are each independently oval-like with through holes and/or blind holes Shaped particles, and the average pore diameter of the first active material is larger than the average pore diameter of the second active material.
  • Fig. 1 is a schematic diagram of the structure of a negative electrode as an example.
  • the negative electrode includes a negative electrode current collector 521, a first active material layer 522 formed on the negative electrode current collector 521, and a second active material layer 523 formed on the surface of the first active material layer 522 away from the negative electrode current collector 521.
  • the composite layer structure negative electrode membrane including the first active material layer and the second active material layer can be formed on one side surface of the negative electrode current collector, or can be formed on two opposite sides of the negative electrode current collector in the thickness direction of the negative electrode current collector. surface.
  • through hole refers to a hole that penetrates the active material particles.
  • blind hole refers to a hole that extends inward to a predetermined depth from the surface of the active material particle, but does not penetrate the active material particle.
  • the first active material and the second active material are each independently oval-like particles with through holes and/or blind holes, in other words, the first active material is an oval-like particle, and it has The porous structure includes one or more of through holes and blind holes; the second active material is an oval-like particle, and it has a porous structure including one or more of through holes and blind holes.
  • the selection of the morphology and pore structure of the first active material and the selection of the morphology and pore structure of the second active material are independent of each other.
  • Exemplary test methods for the average pore diameter of active materials can refer to the standard GB/T19587-2017 "Gas adsorption BET method to determine the specific surface area of solid materials", GB/T21650.2-2008 mercury intrusion method and gas adsorption method to determine the pore size distribution of solid materials and Porosity-Part 2: Gas adsorption analysis of mesopores and macropores.
  • the American Micromeritics TriStar II 3020 instrument can be used to test the average pore size of the active material particles.
  • the inventor found that the negative electrode adopts a composite layer structure of the negative electrode film, and the first active material in the first active material layer and the second active material in the second active material layer use elliptical particles, thus It can improve the accumulation performance between particles, make good contact between particles, and at the same time form pores suitable for electrolyte infiltration.
  • the first active material and the second active material also have a porous structure including one or more of through holes and blind holes, and the second active material layer far from the negative electrode current collector adopts a second active material with a smaller average pore diameter
  • the first active material layer close to the negative electrode current collector adopts the first active material with a larger average pore size. This combined structural feature can greatly increase the liquid absorption and liquid storage capacity of the negative electrode itself.
  • the negative electrode of the present application can significantly alleviate the cycle deterioration caused by insufficient electrolyte infiltration on the premise that the secondary battery adopting it has a higher energy density, and improve the cycle life of the battery. More preferably, the negative electrode of the present application not only maintains high electronic conductivity, but also improves its active ion transport performance, so that the battery can also have excellent dynamic performance.
  • the inventor also found that when the negative electrode adopts a composite layer structure of the negative electrode membrane, the problem of cracking of the active material layer can also be effectively improved.
  • the reason is that two or more active material layers are coated layer by layer, which reduces the internal stress of the active material layer during the drying process of the negative electrode, thereby solving the problem of cracking caused by the increase in coating weight.
  • a continuous conductive network is formed in the negative electrode membrane, which can further improve the cycle life and dynamic performance of the battery.
  • the porosity of the first active material is greater than the porosity of the second active material.
  • the inventor found that the first active material used in the first active material layer of the inner layer has a larger average pore size and a higher porosity, so that the first active material layer has stronger liquid absorption and retention for the electrolyte. .
  • the second active material used in the second active material layer is more dense, with a smaller average pore size and lower porosity, which can ensure that the negative electrode has a higher energy density, and at the same time further improve the negative electrode's liquid storage capacity.
  • the negative electrode can maintain a relatively high electrolyte retention when its volume expands during the cycle. Therefore, the use of the negative electrode can further improve the cycle performance of the battery under the premise of a higher energy density. More preferably, the dynamic performance of the battery can also be improved.
  • the average particle size D v 50 is the particle size corresponding to the cumulative volume distribution percentage of particles reaching 50%.
  • the particles with a larger average particle size D v 50 are more loosely arranged, which can increase the liquid storage rate of the pole piece, but will affect the electronic conductivity between the particles.
  • the average particle size D v 50 of the first active material is preferably 8 ⁇ m-18 ⁇ m, more preferably 10 ⁇ m-16 ⁇ m.
  • the D v 50 of the first active material is in an appropriate range, which can improve the negative electrode’s ability to absorb and store liquid, and at the same time make the negative electrode have higher active ion and electron transport performance, so that the battery has a higher cycle life and power Learn performance.
  • the first active material has an appropriate D v 50, which can also increase the proportion of the active material in the first active material layer per unit volume, thereby helping to increase the energy density of the battery.
  • the average particle size D v 50 of the second active material is preferably 5 ⁇ m-15 ⁇ m, more preferably 6 ⁇ m-12 ⁇ m.
  • the second active material layer adopts a second active material with an appropriate D v 50, which can improve the liquid retention capacity of the negative electrode and at the same time increase the energy density of the negative electrode.
  • the smaller the D v 50 of the second active material is the more fully the contact with the electrolyte is, the more favorable the charge exchange between the active ions and the electrons, and the faster the battery is charged.
  • the D v 50 of the second active material is within an appropriate range, which is also conducive to preparing an active material layer with higher consistency, thereby improving the cycle life of the battery.
  • the negative electrode simultaneously satisfies that the average particle size D v 50 of the first active material is 8 ⁇ m-18 ⁇ m, and the average particle size D v 50 of the second active material is 5 ⁇ m-15 ⁇ m.
  • the size of the active material particles of the first active material layer and the second active material layer have a reasonable combination, which can maintain the stability of the particle accumulation structure during the circulation process, thereby not only preventing the particles between adjacent active material layers from mixing It can also maintain the proper pore structure between the active material particles, thereby effectively exerting the effect of the composite layer structure of the negative electrode membrane on the negative electrode liquid absorption and storage capacity and active ion transport performance. Therefore, the battery adopting the negative electrode can have higher cycle performance and dynamic performance.
  • the electrolyte is also easy to fully contact with the active material with large pore size, which facilitates the deintercalation of active ions and improves the dynamic performance.
  • the use of an active material with a smaller average pore size is beneficial to increase the proportion of the active material per unit volume of the active material layer, thereby increasing the energy density of the negative electrode.
  • the average pore size of the first active material may be 60nm-150nm, preferably 70nm-140nm, more preferably 80nm-120nm.
  • the average pore diameter of the first active material is within an appropriate range, which can better improve the liquid absorption capacity and dynamic performance of the negative electrode.
  • the average pore size of the second active material may be 5nm-35nm, preferably 10nm-30nm, more preferably 15nm-25nm. Within an appropriate range of the average pore diameter of the second active material, the negative electrode can have a higher liquid holding capacity while increasing the energy density.
  • the average pore size of the first active material may be 60nm-150nm, preferably 70nm-140nm, more preferably 80nm-120nm; and the average pore size of the second active material may be 5nm-35nm, preferably 10nm-30nm, more preferably 15nm-25nm.
  • the first active material layer close to the negative electrode current collector selects the first active material with a larger average pore size, which is beneficial to use the capillary action to make the electrolyte quickly infiltrate the negative electrode, improve the liquid absorption rate of the negative electrode piece, and at the same time, keep away from the negative electrode current collector.
  • the second active material layer selects a second active material with a smaller average pore size, and the smaller porosity of the second active material layer helps improve the liquid storage capacity of the negative electrode.
  • the elliptical particles are also spherical particles, and the outer edge surface of the particles is roughly a three-dimensional curved surface.
  • the ratio of the length of the short diameter to the length of the long diameter of the oval-shaped active material particles is ⁇ 1. The closer the value is to 1, the more round the particle shape is, and the greater the shear force between particles. The smaller the ratio of the length of the short diameter to the length of the long diameter, the more the shape of the pellets tends to be elliptical, and the easier it is for the particles to fit into each other.
  • the ratio of the length of the short diameter to the length of the long diameter of the first active material may be 0.4-1, preferably 0.5-1, more preferably 0.6-0.9.
  • the ratio of the length of the short diameter to the length of the long diameter of the first active material is within an appropriate range, which can make good contact between the particles, ensure the higher electronic conductivity of the negative electrode, and increase the porosity of the first active material layer, thereby increasing The amount of electrolyte infiltration of the negative electrode.
  • the ratio of the length of the short diameter to the length of the long diameter of the second active material is 0.3-1, preferably 0.4-0.8.
  • the ratio of the length of the short diameter to the length of the long diameter of the first active material is within an appropriate range, which enables the formation of pores between the particles suitable for electrolyte infiltration, and increases the compactness of the particles, thereby improving the electrolyte retention and energy of the negative electrode density.
  • the negative electrode simultaneously satisfies: the ratio of the short diameter to the long diameter of the first active material is 0.5-1, preferably 0.6-0.9; and the ratio of the short diameter to the long diameter of the second active material is 0.3 -1, preferably 0.4-0.8. Selecting an active material with a larger ratio of short diameter to long diameter to be placed on the negative current collector, and selecting an active material with a small ratio of short diameter to long diameter to be placed on the first active material layer is beneficial Further improve the liquid absorption and storage capacity of the negative electrode.
  • the specific surface area of the active material particles the stronger the adsorption capacity of the electrolyte.
  • the specific surface area of the first active material is greater than the specific surface area of the second active material. This helps to improve the battery's liquid absorption capacity and liquid storage capacity.
  • the specific surface area of the first active material is preferably 6.9m 2 /g-9.6m 2 /g, more preferably 7.5m 2 /g-9.1m 2 /g, especially preferably 8.0m 2 /g- 8.7m 2 /g.
  • the second active substance is preferably a specific surface area of 1.3m 2 /g-3.1m 2 / g, more preferably 2.0m 2 /g-2.5m 2 / g.
  • the apparent density value is the ratio of the mass of the material to the volume of water discharged by the material. The smaller the apparent density value, the larger the volume of open pores contained in the material, and the stronger the liquid absorption and storage capacity.
  • the apparent density value is in the proper range, which is also conducive to making the battery obtain a higher energy density.
  • the apparent density of the first active material is preferably 0.5 g/cm 3 -1.2 g/cm 3 , more preferably 0.6 g/cm 3 -1.0 g/cm 3 .
  • the apparent density of the second active material is preferably 1.5 g/cm 3 -2.0 g/cm 3 , more preferably 1.6 g/cm 3 -1.9 g/cm 3 .
  • the area density of each active material layer is within an appropriate range, which can further improve the energy density and cycle life of the battery. In addition, it also helps to improve the uniformity of the negative electrode.
  • the area density of each active material layer is equal to the mass of the active material layer divided by its area.
  • the surface density of the first active material layer is preferably 20g / m 2 -100g / m 2 , more preferably 30g / m 2 -90g / m 2 .
  • the surface density of the second active material layer is preferably 20g / m 2 -100g / m 2 , more preferably 30g / m 2 -90g / m 2 .
  • the inventor further researched and found that when the ratio of the areal density of the first active material layer to the areal density of the second active material layer is 0.3-3, the energy density and cycle performance of the battery can be further improved. More preferably, the ratio of the areal density of the first active material layer to the areal density of the second active material layer is 0.5-2.
  • the porosity of the negative electrode membrane of the composite layer structure can be 40.1%-67.9%, for example, 44.5%, 45.4%, 50%, 55%, 59.9%, 60.5%, 62.5%, 64.5%, 65.2 %, 66.5%, 67.9%, etc.
  • the negative electrode membrane of the composite layer structure can have an appropriate porosity.
  • the secondary battery using the negative electrode can simultaneously take into account higher energy density and cycle performance.
  • the second active material and the first active material are each independently selected from materials capable of receiving and extracting lithium ions.
  • Materials that can receive and extract lithium ions can include one or more of soft carbon, hard carbon, artificial graphite, natural graphite, silicon, silicon-oxygen compounds, silicon-carbon composites, lithium titanate, and metals that can form alloys with lithium. kind.
  • the second active material and the first active material are both artificial graphite.
  • An exemplary preparation method of artificial graphite as the second active material includes: uniformly mixing artificial graphite particles with an intercalating agent that can decompose and release gas, and the mass ratio of the intercalating agent in the resulting mixture is greater than 0% and less than or equal to 5 %; Carry out the intercalation reaction at about 100°C for 1h ⁇ 3h, such as 2h; make the intercalation agent be embedded between the graphite particles; then transfer the reaction product to the sintering furnace, and sinter at 800°C-1000°C in a protective atmosphere for 8h- 10h, you can get the active material particles.
  • the intercalating agent can be selected from, but not limited to, one or more of lithium carbonate, sodium carbonate, potassium carbonate, ammonium nitrate, lithium chlorate, ammonium oxalate, and acetic acid.
  • a similar method can be used to prepare artificial graphite as the first active material, wherein the first active material can obtain a larger average pore size by increasing the amount of intercalation agent that can decompose and release gas. Furthermore, the first active material can also obtain a higher porosity. For example, in a mixture of artificial graphite particles and an intercalating agent that can decompose and release gas, the mass ratio of the intercalating agent may be 15%-35%.
  • the negative electrode current collector can be made of metal foil, carbon-coated metal foil or porous metal plate, and preferably copper foil.
  • the first active material layer and the second active material layer may each independently include a conductive agent.
  • the conductive agent may include one or more of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
  • the first active material layer and the second active material layer may each independently include a binder.
  • This application does not specifically limit the type of binder, and can be selected according to actual needs.
  • the binder may be one or more of styrene-butadiene rubber (SBR), styrene-butadiene rubber (SBCs), and water-based acrylic resin.
  • the first active material layer and the second active material layer may each independently include a thickening agent, such as sodium carboxymethyl cellulose (CMC-Na).
  • a thickening agent such as sodium carboxymethyl cellulose (CMC-Na).
  • CMC-Na sodium carboxymethyl cellulose
  • this application is not limited to this, and this application can also use other materials that can be used as a thickener for the negative electrode.
  • the average particle size D v 50 of the active material can be conveniently measured with a laser particle size analyzer, such as the Mastersizer 3000 laser particle size analyzer of Malvern Instruments Co., Ltd., UK.
  • a laser particle size analyzer such as the Mastersizer 3000 laser particle size analyzer of Malvern Instruments Co., Ltd., UK.
  • the specific surface area of the active material is a well-known meaning in the art, and it can be measured by instruments and methods known in the art. For example, it can be measured by the nitrogen adsorption specific surface area analysis test method and calculated by the BET (Brunauer Emmett Teller) method, where nitrogen
  • the adsorption specific surface area analysis test can be performed by the TriStar II specific surface and pore analyzer of Micromeritics, USA. The test can refer to GB/T 19587-2004.
  • the apparent density of the active material can be measured using instruments and methods known in the art. For details, please refer to the national standard GB/T24586-2009 for determination of apparent density, true density and porosity of iron ore.
  • true volume particle weight/true density
  • the true density can be measured by a true density tester (such as AccuPyc II 1340).
  • the ratio of the length of the short axis to the length of the long axis of the active material can be determined by using instruments and methods known in the art.
  • a second aspect of the present application provides a secondary battery, which includes a positive electrode, a negative electrode, an electrolyte, and a separator, wherein the negative electrode is the negative electrode according to the first aspect of the present application.
  • the positive electrode includes a positive electrode current collector, a positive electrode membrane provided on at least one surface of the positive electrode current collector and including a positive electrode active material.
  • the specific type and composition of the positive pole piece are not specifically limited, and can be selected according to actual needs.
  • the positive electrode active material is selected from, but not limited to, layered lithium transition metal oxides with the chemical formula Li a M 1-x M'x O 2 and the chemical formula LiFe y Mn 1-yz M" z PO 4 / One or a mixture of C b lithium iron phosphate materials, where 0.9 ⁇ a ⁇ 1.1, 0 ⁇ x ⁇ 0.1, 0.1 ⁇ y ⁇ 0.9, 0 ⁇ z ⁇ 0.9, b ⁇ 0, M is Co, At least one of Mn and Ni, M'is one of Al, Mg, B, Zr, Si, Ti, Cr, Fe, V, Cu, Ca, Zn, Nb, Mo, Sr, Sb, W, and Bi Or several, M" is one or several of Cr, Mg, Ti, Al, Zn, W, Nb, Zr.
  • the positive electrode membrane may optionally include a conductive agent.
  • a conductive agent may include one or more of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
  • the positive electrode membrane may optionally include a binder.
  • a binder may include one or more of polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), ethylene-vinyl acetate copolymer (EVA), and polyvinyl alcohol (PVA).
  • PVDF polyvinylidene fluoride
  • PTFE polytetrafluoroethylene
  • EVA ethylene-vinyl acetate copolymer
  • PVA polyvinyl alcohol
  • the positive electrode current collector can be a metal foil, a carbon-coated metal foil or a porous metal plate, preferably an aluminum foil.
  • the electrolyte includes a solvent and a solute.
  • the specific type and composition of the solvent and the solute are not specifically limited, and can be selected according to actual needs.
  • the solvent can be selected from one or more of organic carbonates such as ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, etc., which are electrically insulating but can conduct ions .
  • the solute can be selected from one or more lithium salts of LiPF 6 , LiBF 4 , LiBOB, LiAsF 6 , Li(CF 3 SO 2 ) 2 N, LiCF 3 SO 3 , and LiClO 4 .
  • the separator is interposed between the positive pole piece and the negative pole piece for isolation.
  • the type of the separator is not specifically limited, and it can be any separator material used in existing batteries.
  • Fig. 2 shows a secondary battery 5 with a square structure as an example.
  • the secondary battery may include an outer package for packaging the positive pole piece, the negative pole piece, the separator and the electrolyte.
  • the outer packaging of the secondary battery may be a soft bag, such as a pouch type soft bag.
  • the material of the soft bag can be plastic, for example, it can include one or more of polypropylene PP, polybutylene terephthalate PBT, polybutylene succinate PBS, and the like.
  • the outer packaging of the secondary battery may also be a hard shell, such as a hard plastic shell, aluminum shell, steel shell, and the like.
  • the outer package may include a housing 51 and a cover 53.
  • the housing 51 may include a bottom plate and a side plate connected to the bottom plate, and the bottom plate and the side plate enclose a receiving cavity.
  • the housing 51 has an opening communicating with the containing cavity, and a cover plate 53 can cover the opening to close the containing cavity.
  • the positive pole piece, the negative pole piece and the separator may be laminated or wound to form a laminated structure electrode assembly or a wound structure electrode assembly 52.
  • the electrode assembly 52 is packaged in the receiving cavity.
  • the electrolyte is infiltrated in the electrode assembly 52.
  • the number of electrode assemblies 52 included in the secondary battery 5 can be one or several, which can be adjusted according to requirements.
  • the secondary battery can be assembled into a battery module, and the number of secondary batteries contained in the battery module can be multiple, and the specific number can be adjusted according to the application and capacity of the battery module.
  • Fig. 4 is a battery module 4 as an example.
  • a plurality of secondary batteries 5 may be arranged in sequence along the length direction of the battery module 4. Of course, it can also be arranged in any other manner. Furthermore, the plurality of secondary batteries 5 can be fixed by fasteners.
  • the battery module 4 may further include a housing having an accommodation space, and a plurality of secondary batteries 5 are accommodated in the accommodation space.
  • the above-mentioned battery modules can also be assembled into a battery pack, and the number of battery modules contained in the battery pack can be adjusted according to the application and capacity of the battery pack.
  • FIGS 5 and 6 show the battery pack 1 as an example.
  • the battery pack 1 may include a battery box and a plurality of battery modules 4 disposed in the battery box.
  • the battery box includes an upper box body 2 and a lower box body 3.
  • the upper box body 2 can be covered on the lower box body 3 and forms a closed space for accommodating the battery module 4.
  • Multiple battery modules 4 can be arranged in the battery box in any manner.
  • a device in a third aspect of the present application, includes the secondary battery of the second aspect of the present application.
  • the secondary battery can be used as a power source of the device, and can also be used as an energy storage unit of the device.
  • the device can be, but is not limited to, mobile devices (such as mobile phones, laptop computers, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf Vehicles, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc.
  • the device can select a secondary battery, battery module, or battery pack according to its usage requirements.
  • Fig. 7 is a device as an example.
  • the device is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle.
  • a battery pack or battery module can be used.
  • the device may be a mobile phone, a tablet computer, a notebook computer, etc.
  • the device is generally required to be thin and light, and a secondary battery can be used as a power source.
  • the batteries of Examples 1-19 and Comparative Examples 1 and 2 were prepared according to the following methods.
  • the linear speed of stirring is controlled at 4-10m/min, and the stirring and mixing time is 60-150min, until the system is uniform, and the cathode slurry is obtained;
  • the positive pole pieces are obtained by drying, cold pressing, slitting and cutting.
  • the negative electrode active material, conductive carbon black Super-P, binder styrene-butadiene rubber (SBR), and thickener sodium carboxymethyl cellulose (CMC-Na) shown in Table 1 in Comparative Examples 1 and 2 are in a weight ratio 96:1:2:1 for mixing. After fully stirring and mixing in a deionized water solvent system, a negative electrode slurry is obtained; the negative electrode slurry is evenly coated on both surfaces of the negative electrode current collector Cu foil, refer to The areal densities shown in Comparative Examples 1 and 2 in Table 1 were coated, dried at room temperature and then transferred to an oven to continue drying, and then cold-pressed and slit to obtain negative pole pieces.
  • SBR binder styrene butadiene rubber
  • CMC-Na thickener sodium carboxymethyl cellulose
  • SBR binder styrene butadiene rubber
  • CMC-Na thickener sodium carboxymethyl cellulose
  • the slurry A was uniformly coated on the two surfaces of the negative current collector Cu foil, and the coating was carried out with reference to the areal density shown in Examples 1-19 in Table 1. After drying at room temperature, it was transferred to an oven to continue drying. Obtain the pole piece A coated with the first active material layer; then coat the slurry B on both surfaces of the pole piece A, refer to the areal density shown in Examples 1-19 in Table 1, for coating, and bake Dry, then cold press and slit to obtain a negative electrode with two active material layers.
  • the graphite in Table 1 is all artificial graphite.
  • the lithium ion secondary battery made by the negative electrode obtained in Examples 1-19 and Comparative Examples 1 and 2 was subjected to a current of 0.5C (that is, the current value of completely discharging the theoretical capacity within 2h).
  • the charging is constant current and constant voltage charging
  • the charge termination voltage is 4.2V
  • the cut-off current is 0.05C
  • the discharge termination voltage is 3.0V
  • the BOL (Before of life) of the battery is the discharge capacity C b at the first cycle.
  • the test condition is 1C/1C cycle under normal temperature conditions, the voltage range is 3.0V-4.2V, the middle is left for 5min, and the discharge capacity C e is recorded during each cycle.
  • the ratio of C e to C b , C e /C b is the capacity retention rate during this cycle. Test the capacity retention rate of the battery after 2000 cycles.
  • Example 1-19 and Comparative Examples 1 and 2 The related parameters of the negative electrodes provided in Examples 1-19 and Comparative Examples 1 and 2 are shown in Table 1, and the negative electrode test results provided in Examples 1-19 and Comparative Examples 1 and 2 are shown in Table 2, and Examples 1-19 and Comparative Example 1 , 2 The test results of the secondary battery prepared with the negative electrode provided are shown in Table 3.
  • Examples 1-18 of the present application adopt a composite layer structure of the negative electrode film, wherein the first active material layer and the second active material layer in the first active material layer
  • the second active material is elliptical particles with through holes and/or blind holes, and the average pore diameter of the first active material is larger than the average pore diameter of the second active material, thereby enabling the negative electrode to have good active material particles While stacking performance, it greatly increases its own liquid absorption and storage capacity, so that the secondary battery adopting it has a higher energy density and improves the cycle life.
  • Examples 1-7 show that by changing the average pore size of the first active material, its apparent density and specific surface area will change accordingly, especially affecting the pole piece liquid absorption and liquid retention performance and circulation capacity. It can also be seen that the average pore size is preferably controlled at 70nm-140nm, more preferably 80nm-120nm, which can further improve the liquid absorption and liquid retention capacity of the negative electrode, thereby further improving the cycle performance of the battery.
  • the average pore size of the second active material is preferably controlled in the range of 10nm-30nm, more preferably 15nm-25nm, which can further improve the liquid absorption and retention capacity of the negative electrode and further improve the cycle performance of the battery.

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Abstract

L'invention concerne une électrode négative et une batterie secondaire et un dispositif les comprenant. L'électrode négative comprend : un collecteur de courant ; une première couche de matériau actif comprenant un premier matériau actif et positionnée à proximité du collecteur de courant ; et une seconde couche de matériau actif comprenant un second matériau actif et disposée au niveau d'une surface de la première couche de matériau actif à distance du collecteur de courant. Le premier matériau actif et le second matériau actif sont des particules ovoïdes indépendantes comportant un trou traversant et/ou un trou borgne. Le diamètre de trou moyen du premier matériau actif est supérieur au diamètre de trou moyen du second matériau actif.
PCT/CN2020/078166 2019-03-06 2020-03-06 Électrode négative et batterie secondaire et dispositif les comprenant WO2020177760A1 (fr)

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EP22168100.0A EP4047681B1 (fr) 2019-03-06 2020-03-06 Électrode négative, batterie secondaire et dispositif les comprenant
EP20766175.2A EP3800706B1 (fr) 2019-03-06 2020-03-06 Électrode négative et batterie secondaire et dispositif les comprenant
US17/150,096 US11600816B2 (en) 2019-03-06 2021-01-15 Negative electrode, secondary battery and device comprising same
US18/103,531 US20230170474A1 (en) 2019-03-06 2023-01-31 Negative electrode, secondary battery and device comprising same

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CN201910169334.4A CN111668452B (zh) 2019-03-06 2019-03-06 一种负极及其锂离子二次电池

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CN111668452B (zh) 2021-06-04
EP3800706B1 (fr) 2022-06-01
US20210143414A1 (en) 2021-05-13
CN111668452A (zh) 2020-09-15
US20230170474A1 (en) 2023-06-01
US11600816B2 (en) 2023-03-07

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